Miscibility Gap Closure, Interface Morphology, and Phase Microstructure of 3D LixFePO 4 Nanoparticles from Surface Wetting and Coherency Strain
We study the mesoscopic effects which suppress phase-segregation in LixFePO4 nanoparticles using a multiphysics phase-field model implement on a high performance cluster. We simulate 3D spherical particles of radii from 3nm to 40nm and examine the equilibrium microstructure and voltage profiles as a they depend on size and overall lithiation. The model includes anisotropic, concentration-dependent elastic moduli, misfit strain, and facet dependent surface wetting within a Cahn-Hilliard formulation. Here, we find that the miscibility gap vanishes for particles of radius ~ 5 nm, and the solubility limits change with overall particle lithiation. The corresponding voltage plateau, indicative of phase-segregation, changes in extent and also vanishes. Surface wetting is found to have a strong effect on stabilizing a variety of microstructures, exaggerating the shifting of solubility limits, and shortening the voltage plateau.
- Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
- Univ. of Chicago, IL (United States). Computation Inst.
- Northwestern Univ., Evanston, IL (United States). McCormick School of Engineering
- Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Univ. of Chicago, IL (United States). Computation Inst.
- Publication Date:
- OSTI Identifier:
- Grant/Contract Number:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 10; Journal ID: ISSN 1936-0851
- American Chemical Society (ACS)
- Research Org:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); US Department of Commerce
- Country of Publication:
- United States
- 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY Li-ion battery; LiFePO4; coherency strain; interface morphology; nanoparticles; phase-field model; surface wetting
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